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  • 1Department of Organic Chemistry I, University of the Basque Country UPV/EHU , Avenida de Tolosa 72, 20018 San Sebastian, Spain.

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Buckyballs (C60 fullerenes) show hydrophobic solvation but not hydrophobic interactions in water. Molecular dynamics simulations reveal distinct interfacial water structures that explain this behavior, challenging typical hydrophobic interaction theories.

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Area of Science:

  • Physical Chemistry
  • Supramolecular Chemistry
  • Materials Science

Background:

  • Buckyballs (C60 fullerenes) exhibit contradictory properties: insolubility in water (hydrophobic) yet repulsive solvent-induced interactions.
  • Understanding the behavior of fullerenes in aqueous environments is crucial for their application in various fields.

Purpose of the Study:

  • To reconcile the opposing observations of buckyball hydrophobicity and repulsive interactions in water.
  • To investigate the role of interfacial water structure in the association of C60 fullerenes.

Main Methods:

  • Molecular dynamics simulations of C60 fullerene association in water at varying temperatures.
  • Comparison with simulations in nonpolar solvents and with graphene sheet association.

Main Results:

  • Enthalpy and entropy changes for fullerene association in water were small and temperature-independent, contradicting typical hydrophobic interactions.
  • Distinct interfacial water structures between associated buckyballs were identified, characterized by lower entropy, density, and hydrogen bonding.
  • These distinct waters oppose the liberation of bulk water, explaining the non-hydrophobic effective pair interaction.

Conclusions:

  • Buckyballs display hydrophobic solvation properties but not hydrophobic pair interactions due to unique interfacial water structures.
  • Hydrophobic solvation and hydrophobic interactions are not always directly correlated, especially for convex solutes like fullerenes.
  • Buckyballs serve as a model system where hydrophobic solvation cannot be inferred from hydrophobic interaction.